环境科学学报2025,Vol.45Issue(1) :461-469.DOI:10.13671/j.hjkxxb.2024.0297

温度对NO2参与非均相反应生成硫酸盐颗粒物的影响研究

Effect of temperature on the participation of NO2 in heterogeneous reaction to form sulfate particulate matter

杨子墨 何翔 王双喜 杨超群 陈星雨
环境科学学报2025,Vol.45Issue(1) :461-469.DOI:10.13671/j.hjkxxb.2024.0297

温度对NO2参与非均相反应生成硫酸盐颗粒物的影响研究

Effect of temperature on the participation of NO2 in heterogeneous reaction to form sulfate particulate matter

杨子墨 1何翔 1王双喜 1杨超群 1陈星雨1
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作者信息

  • 1. 新疆大学生态与环境学院,乌鲁木齐 830017;绿洲生态教育部重点实验室,乌鲁木齐 830017;新疆精河温带荒漠生态系统教育部野外科学观测研究站,乌鲁木齐 830017
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摘要

采用原位漫反射傅里叶变换光谱技术研究了SO2/NO2在α-Fe2O3颗粒物表面的非均相反应,探究了温度对NO2参与非均相反应生成硫酸盐颗粒物的影响.结果表明,硫酸盐(1259、1159、1069 cm-1)和硝酸盐(1603、1414、1335 cm-1)的特征峰在颗粒物表面生成.NO2促进了吸附态SO2生成硫酸盐,而N2O4是生成硫酸盐的关键氧化剂.随着温度由253 K增加到298 K,SO2/NO2在α-Fe2O3颗粒物表面的反应速率降低了65%左右,同时反应初始阶段的摄取系数由(4.88±0.07)×10-7降低到(3.42±0.04)×10-7.表明温度的变化对SO2/NO2在α-Fe2O3颗粒物表面的非均相反应具有显著影响,并且在低温条件下,α-Fe2O3颗粒物对反应初始阶段SO2具有更大的摄取能力,有助于解释冬季硫酸盐颗粒物的爆发性增长的现象.

Abstract

Heterogeneous reactions of SO2/NO2 on the surface of α-Fe2O3 particles were investigated by in situ diffuse reflection Fourier transform spectroscopy.The influence of temperature on the formation of sulfate particles by NO2 participating in heterogeneous reactions was investigated.The results showed that characteristic peaks of sulfate(1259,1159,1069 cm-1)and nitrate(1603,1414,1335 cm-1)were formed on the surface of the particles.NO2 promoted the formation of sulfate from adsorbed SO2,while surface N2O4 was the key oxidant for sulfate formation.As the temperature increased from 253 K to 298 K,the reaction rate of heterogeneous reaction decreased by about 65%,and the initial uptake coefficient decreased from(4.88±0.07)×10-7 to(3.42±0.04)×10-7.The results showed that the temperature change exhibited a significant effect on the heterogeneous reaction of SO2/NO2 on the surface of α-Fe2O3 particles,α-Fe2O3 particles exhibited a greater uptake of SO2 at the initial stage of the reaction and at low temperature,which helped to explain the explosive growth of sulfate particles in winter.

关键词

非均相反应/温度/NO2/α-Fe2O3颗粒物/硫酸盐

Key words

heterogeneous reaction/temperature/NO2/α-Fe2O3 particles/sulfate

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出版年

2025
环境科学学报
中国科学院生态环境研究中心

环境科学学报

北大核心
影响因子:1.645
ISSN:0253-2468
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